Analyzing data from our optical dust logger, we find that volcanic ash layers from the Siple Dome (Antarctica) borehole are simultaneous (with >99% rejection of the null hypothesis) with the onset of millennium-timescale cooling recorded at Greenland Ice Sheet Project 2 (GISP2; Greenland). These data are the best evidence yet for a causal connection between volcanism and millennial climate change and lead to possibilities of a direct causal relationship. Evidence has been accumulating for decades that volcanic eruptions can perturb climate and possibly affect it on long timescales and that volcanism may respond to climate change. If rapid climate change can induce volcanism, this result could be further evidence of a southern-lead North-South climate asynchrony. Alternatively, a volcanic-forcing viewpoint is of particular interest because of the high correlation and relative timing of the events, and it may involve a scenario in which volcanic ash and sulfate abruptly increase the soluble iron in large surface areas of the nutrient-limited Southern Ocean, stimulate growth of phytoplankton, which enhance volcanic effects on planetary albedo and the global carbon cycle, and trigger northern millennial cooling. Large global temperature swings could be limited by feedback within the volcano-climate system.